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Synthesis, characterization and catalytic activity of transition metal ...

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ash in an alkaline solution, followed by crystallisation to form the ring like structures that are<br />

necessary for zeolite construction. The high percentage <strong>of</strong> aluminosilicates in fly ash makes them<br />

a cheap <strong>and</strong> readily available source <strong>of</strong> Si <strong>and</strong> Al for zeolite synthesis. The low Si/Al ratio <strong>of</strong> fly<br />

ash allows for the synthesis <strong>of</strong> low Si zeolites, which have a high cation exchange capacity, high<br />

affinity towards polar molecules <strong>and</strong> a large pore volume [16].<br />

Homogeneous catalysts can <strong>of</strong>fer high molar <strong>catalytic</strong> efficiencies <strong>and</strong> rates under mild<br />

conditions, tolerance to many types <strong>of</strong> organic functionality <strong>and</strong> high selectivity in reactions that<br />

allow formation <strong>of</strong> specific desired reaction product. Heterogeneous catalysts are usually more<br />

robust (insensitive to air <strong>and</strong> moisture), easy to h<strong>and</strong>le <strong>and</strong> can be completely removed from the<br />

reaction easily. An ideal catalyst would possess the beneficial aspects <strong>of</strong> both homogeneous <strong>and</strong><br />

heterogeneous systems. Towards this objective, significant work has been exp<strong>and</strong>ed in an attempt<br />

to develop homogeneous catalysts that have been anchored to a solid support though it is<br />

associated with multiple practical difficulties. Encapsulation <strong>of</strong> <strong>transition</strong> <strong>metal</strong> complexes in<br />

zeolites <strong>and</strong> related materials has gained much attention since they possess both homogeneous <strong>and</strong><br />

heterogeneous <strong>catalytic</strong> characters. The rigid inorganic zeolite framework defines the reaction<br />

cavity surrounding the active sites <strong>of</strong> the <strong>transition</strong> <strong>metal</strong> complexes. Though the encapsulation <strong>of</strong><br />

<strong>transition</strong> <strong>metal</strong> complexes in zeolites have been established as good catalysts, the replacement <strong>of</strong><br />

commercial zeolites by FAZ has gained only little attention. Recently, encapsulation <strong>of</strong> N,N′-<br />

ethylenebis(salicylamide) <strong>metal</strong> complexes in fly ash based zeolite was reported <strong>and</strong> these<br />

complexes have been found to catalyze the liquid phase hydroxylation <strong>of</strong> phenol with hydrogen<br />

peroxide [17]. Up to now, hydroxylation <strong>of</strong> phenol with hydrogen peroxide as the oxidant has<br />

become the most general way to obtain diphenols owing to its environmental acceptability. The<br />

<strong>activity</strong> <strong>of</strong> the encapsulated <strong>transition</strong> <strong>metal</strong> complexes is different from that <strong>of</strong> the neat<br />

complexes since the selectivity is altered in a constrained environment [18-20] Results from the<br />

present study seems promising enough to introduce the <strong>transition</strong> <strong>metal</strong> complexes encapsulated<br />

zeolites as catalysts for the liquid phase hydroxylation <strong>of</strong> phenol. However, more investigations<br />

are recommended to confirm the industrial applicability <strong>of</strong> the obtained results, especially<br />

concerning the total efficiency <strong>and</strong> economics.<br />

This work involves the (i) the synthesis <strong>of</strong> zeolite from fly ash (ii) characterisation <strong>of</strong> the<br />

synthesized FAZ (iii) encapsulation <strong>of</strong> <strong>transition</strong> <strong>metal</strong>-ascorbate complexes in the zeolite cavities<br />

4

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